US3048647A - Separator media for aluminum cells - Google Patents

Separator media for aluminum cells Download PDF

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Publication number
US3048647A
US3048647A US718141A US71814158A US3048647A US 3048647 A US3048647 A US 3048647A US 718141 A US718141 A US 718141A US 71814158 A US71814158 A US 71814158A US 3048647 A US3048647 A US 3048647A
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anode
aluminum
separator
cells
cell
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US718141A
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Margaret P Korver
Nelson C Cahoon
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Union Carbide Corp
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Union Carbide Corp
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    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M6/00—Primary cells; Manufacture thereof
    • H01M6/22—Immobilising of electrolyte
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
    • H01M50/40—Separators; Membranes; Diaphragms; Spacing elements inside cells
    • H01M50/409—Separators, membranes or diaphragms characterised by the material
    • H01M50/411—Organic material
    • H01M50/414—Synthetic resins, e.g. thermoplastics or thermosetting resins
    • H01M50/42—Acrylic resins
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
    • H01M50/40—Separators; Membranes; Diaphragms; Spacing elements inside cells
    • H01M50/409—Separators, membranes or diaphragms characterised by the material
    • H01M50/411—Organic material
    • H01M50/414—Synthetic resins, e.g. thermoplastics or thermosetting resins
    • H01M50/423—Polyamide resins
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
    • H01M50/40—Separators; Membranes; Diaphragms; Spacing elements inside cells
    • H01M50/409—Separators, membranes or diaphragms characterised by the material
    • H01M50/411—Organic material
    • H01M50/429—Natural polymers
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M6/00—Primary cells; Manufacture thereof
    • H01M6/04—Cells with aqueous electrolyte
    • H01M6/06—Dry cells, i.e. cells wherein the electrolyte is rendered non-fluid
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
    • H01M50/40—Separators; Membranes; Diaphragms; Spacing elements inside cells
    • H01M50/46—Separators, membranes or diaphragms characterised by their combination with electrodes

Definitions

  • This invention relates to improved separator means for primary cells utilizing aluminum metal as the anode material, a carbon cathode with an oxidic depolarizer, an aqueous electrolyte, and a paper separator between the anode and the cathode.
  • a number of disadvantages limits the usefulness of cells having aluminum anodes.
  • One disadvantage of such cells is that they have a relatively short shelf life.
  • Another disadvantage of cells using aluminum anodes as compared with LeClanche cells is their poor performance under heavy, light and delayed service. Such cells also often leak or crack before they are electrically spent. Additionally, cells containing aluminum anodes are subject to the accumulation of oxidic film on the anode, thereby preventing instantaneous response for current when put to use.
  • a bibulous ionically-permeable colloidal layer next to the aluminum anode This layer when placed in a cell containing a suitable electrolyte becomes tacky and forms a uniform adhesive bond between the anode and cathode.
  • the colloidal layer in question may be incorporated in cells using aluminum anodes in any one of three different ways.
  • a colloid film may be placed on the anode, and the mix added to the cell.
  • the colloid film may be applied to the bobbin before the same is placed in the container for the cell.
  • a colloid film layer is applied on a paper separator.
  • the powdered colloids found useful in the practice of the invention necessarily are stable-in cell electrolyte, and resistant to chemical deterioration in cell environment.
  • Such colloids include locust bean gum, gum Karaya, and polyacrylamide resins.
  • any colloid which is substantially b-ibulous in electrolytes used in conjunction with aluminum anodes, and is resistant to hydrolysis in such medium is operative in the practice of the present invention.
  • the electrolytes referred to in the preceding paragraph include aluminum chloride, ammonium chromate solutions, aluminum chloride hexahydrate and ammonium, sodium or potassium chromate.
  • the colloidal material is suspended in a resin solution and applied to a paper backing such as a special grade of alpha cellulose, which is high in wet strength.
  • the separator medium may be made to the surface of the aluminum anode or to the surface of the barrier sheet or to both.
  • the aluminum anode coated with a dry anode layer may then be coated with paper or suitable barrier film, and the whole unit fed to a punch press to prepare individual cell anodeseparator units for cell assembly.
  • resins suitable for forming solution for suspending the colloids of the invention by dissolving in low molecular weight solvents are polyvinylacetate and polyvinylformaldehyde.
  • Suitable solvents for the purposes of this invention are acetone, ethyl ether, ethyl alcohol, chloral, chloroform, cyclopentane, heptane, and, in general, low molecular weight alcohols, ketones and ethers which are compatible with the selected colloids, resins and cell electrolyte.
  • composition of the electrolyte influences the choice of colloid, considerable variation in the electrolyte chosen for the aluminum cell is permissible. For example, in an aluminum cell using either MnCl alone or MnCl modified by Na B O locust bean gum has been found to operate satisfactorily.
  • separators of the invention increase the ease of aluminum cell assembly. Where previously soft filter paper was used as a separator, it presented a problem because it ripped easily upon becoming Wet with bobbin moisture, and often caused short-circuited cells. In the practice of the invention, the addition of a colloid to a paper backing tends to give the paper a great deal more strength.
  • a cell having an anode consisting of aluminum and alloys thereof, a depolarizer and an electrolyte selected from the group consisting of aluminum chloride, ammonium chromate, aluminum chloride hexahydrate, sodium chromate and potassium chromate, an ionically permeable separator medium between said anode and said depolarizer, said separator medium consisting of paper backing having bound thereto a colloid bibulous in said electrolyte and resistant to hydrolysis in said electrolyte, said colloid being selected from the group consisting of locust bean gum, gum karaya and polyacrylamide resins and being bound to said paper backing by means of a binder resin.
  • a cell having an anode consisting of aluminum and alloys thereof, and an electrolyte selected from. the group consisting of aluminum chloride, ammonium chr0- mate, aluminum chloride hexahydrate, sodium chromate and potassium chromate, an ionically permeable separator medium bound to said anode, said separator medium comprising a colloid bibulous in said electrolyte and resistant to hydrolysis in said electrolyte, said colloid being selected from the group consisting of locust bean gum, gum karaya and polyacrylamide resins and being bound to the said anode by means of a binder resin.
  • an electrolyte selected from. the group consisting of aluminum chloride, ammonium chr0- mate, aluminum chloride hexahydrate, sodium chromate and potassium chromate, an ionically permeable separator medium bound to said anode, said separator medium comprising a colloid bibulous in said electrolyte and resistant to hydrolysis in said electrolyt

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  • Chemical & Material Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Electrochemistry (AREA)
  • General Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Manufacturing & Machinery (AREA)
  • Cell Separators (AREA)
  • Conductive Materials (AREA)

Description

ilnited States Patent Undue 3,04%,647 Patented Aug. 7, 1962 3,048,647 SEPARATOR MEDEA FUR ALUMRNUM CELLS Margaret P. Korver, Breclrsville, and Nelson C. Cahoon,
Fairview Park, Ohio, assignors to Union Carbide Corporation, a corporation of New York No Drawing. Filed Feb. 28, 1958, Ser. No. 718,141 5 Uaims. (Cl. 136146) This invention relates to improved separator means for primary cells utilizing aluminum metal as the anode material, a carbon cathode with an oxidic depolarizer, an aqueous electrolyte, and a paper separator between the anode and the cathode.
A number of disadvantages limits the usefulness of cells having aluminum anodes. One disadvantage of such cells is that they have a relatively short shelf life. Another disadvantage of cells using aluminum anodes as compared with LeClanche cells, is their poor performance under heavy, light and delayed service. Such cells also often leak or crack before they are electrically spent. Additionally, cells containing aluminum anodes are subject to the accumulation of oxidic film on the anode, thereby preventing instantaneous response for current when put to use.
It has been found, in accordance with the present invention, that the drying out of the separator used with dry cell systems using aluminum metal as the anodic material is to a great extent responsive for the above-enumerated shortcomings of such systems. This is believed to be due to the fact that in drying out, the separator frequently pulls away from the anode, and does not allow the proper necessary electrical contact between the separator and the anode of the cell.
It is, therefore, the principal object of the invention to provide improved separator means for use in dry cells employing aluminum metal as the anode material.
It is a further object of this invention to provide means facilitating the application of a separator to an aluminum anode, and thereby increase the ease of assembling cells using such anodes.
The above objects are attained, in the practice of the invention, by a bibulous ionically-permeable colloidal layer next to the aluminum anode. This layer when placed in a cell containing a suitable electrolyte becomes tacky and forms a uniform adhesive bond between the anode and cathode. The colloidal layer in question may be incorporated in cells using aluminum anodes in any one of three different ways. In one embodiment, a colloid film may be placed on the anode, and the mix added to the cell. Alternatively, the colloid film may be applied to the bobbin before the same is placed in the container for the cell. In the preferred embodiment of the invention, a colloid film layer is applied on a paper separator.
The powdered colloids found useful in the practice of the invention necessarily are stable-in cell electrolyte, and resistant to chemical deterioration in cell environment. Such colloids include locust bean gum, gum Karaya, and polyacrylamide resins. Generally, however, any colloid which is substantially b-ibulous in electrolytes used in conjunction with aluminum anodes, and is resistant to hydrolysis in such medium, is operative in the practice of the present invention.
The electrolytes referred to in the preceding paragraph include aluminum chloride, ammonium chromate solutions, aluminum chloride hexahydrate and ammonium, sodium or potassium chromate.
Suitably in the practice of the invention the colloidal material is suspended in a resin solution and applied to a paper backing such as a special grade of alpha cellulose, which is high in wet strength.
As stated before, application of the separator medium may be made to the surface of the aluminum anode or to the surface of the barrier sheet or to both. In fact, the aluminum anode coated with a dry anode layer may then be coated with paper or suitable barrier film, and the whole unit fed to a punch press to prepare individual cell anodeseparator units for cell assembly.
Any binder resin which when used in appropriate amounts permits the release of the colloid when the anode layer containing such colloid is contacted with cell electrolyte, is operative. Any solvent in which the binder resin is soluble and in which the colloid is neither soluble nor bibulous to an appreciable degree is satisfactory for applying the colloid layer to the paper backing sheet or the anode or both.
Examples of resins suitable for forming solution for suspending the colloids of the invention by dissolving in low molecular weight solvents are polyvinylacetate and polyvinylformaldehyde.
Suitable solvents for the purposes of this invention are acetone, ethyl ether, ethyl alcohol, chloral, chloroform, cyclopentane, heptane, and, in general, low molecular weight alcohols, ketones and ethers which are compatible with the selected colloids, resins and cell electrolyte.
In an embodiment of the invention, 9.52 grams of various colloid-forming materials were suspended each in a solution of 3.0 g. of polyvinyl acetate in -300 cc. of acetone. High wet strength alpha cellulose paper was coated with each of the above colloidal suspensions to give 300 square inches of test separator.
Separators so prepared were placed in an aluminum cell electrolyte having the following composition:
The relative electrolyte absorption by each separator was measured, and is tabulated in Table I below.
TABLE I Relative Absorption of Various Colloidal Materials in Aluminum Chloride Electrolyte Locust Hydroxy Poly- Poly- Absorpbean propyl acryl- Methyl vinyl Karaya tion gum methyl amide cellulose alcohol gum cellulose 1 day 1. 74 0. 0795 2. 41 0.1051 0.0618 4. 00
While it is recognized that the composition of the electrolyte influences the choice of colloid, considerable variation in the electrolyte chosen for the aluminum cell is permissible. For example, in an aluminum cell using either MnCl alone or MnCl modified by Na B O locust bean gum has been found to operate satisfactorily.
A comparison of the service obtained on cells containing these separators with cells using plain filter paper as the separator medium is tabulated in Table II below. It should be noted that all three numbered lots of cells were prepared from, and contained the same quantities of active ingredients, so that the only variable was the separator medium. Service values for standard commercial Zinc LeClanche cells of the same size also are given for comparison purposes in the table. It is apparent from this table that on the very heavy, very light and all delayed service tests, the film-lined cells of lots 2 and 3 excel appreciably. Cells containing filter paper separators perform very poorly under the same service conditions.
TABLE II Eflect of Separator Medium on the Service of Al-MnO Cells 2.25 ohm continuousmin. to 0.65 v. Lot Separator Initial 6 mos. 12 mos.
-1 Filter paper (control) 166 75 N.G. 2 Paper plus locust bean gum 229 252 294 3 Paper plus gum Karaya 249 265 N.G. 4 Zinc cells- 210 4 ohm cntinuous min. to 0 75 v. Lot Separator Initial 6 mos. 12 mos.
Filter paper (control) 469 30 N. G Paper plus locust bean gu 479 469 615 Paper plus gum Karaya 429 382 471 Zinc cells 7.5 ohm contin- Lot Separator u0us min. to 0.85 v initial 1 Filter Paper (control) 265 2 Paper plus locust bean gum 1, 315 3 Paper plus gum Karaya n 4 Zinc cells 4 ohm HIFmin. to 1.1, 0.9, 0.8 v. Lot 15 ohm continuous-min. to
0.85 v., initial Initial 6 months 01111112 2.25 ohm LIF 225 ohm int.- hrs./day min. to 0.05 v. min. to 0.65 v. Lot hrs. to 0.9 v., initial Initial 6 months Initial 6 months 64 301 N.G. 21 35 49 355 289 427 355 3 42 333 357 205 332 Zine cells .n 420 635 4 ohm LIF-min. to 1.1, 0.9, 0.8 v.
Lot
Initial 6 months 12 months Leaders uniform tacky contact of the anode with the cathode is essential for satisfactory output. It is presumed that drying out of the filter paper separator leads to poor service maintenance of cells containing the same. By contrast, good service maintenance is obtained with the colloids of the invention, which provide a moist, lasting, tacky contact between anode and electrolyte.
In addition to improved cell performance, use of the separators of the invention increases the ease of aluminum cell assembly. Where previously soft filter paper was used as a separator, it presented a problem because it ripped easily upon becoming Wet with bobbin moisture, and often caused short-circuited cells. In the practice of the invention, the addition of a colloid to a paper backing tends to give the paper a great deal more strength.
What is claimed is:
1. In a cell having an anode consisting of aluminum and alloys thereof, a depolarizer and an electrolyte selected from the group consisting of aluminum chloride, ammonium chromate, aluminum chloride hexahydrate, sodium chromate and potassium chromate, an ionically permeable separator medium between said anode and said depolarizer, said separator medium comprising a c lloid bibulous in said electrolyte and resistant to hydrolysis in said electrolyte, said colloid being selected from the group consisting of locust bean gum, gum karaya and polyacrylarnide resins.
2. In a cell having an anode consisting of aluminum and alloys thereof, a depolarizer and an electrolyte selected from the group consisting of aluminum chloride, ammonium chromate, aluminum chloride hexahydrate, sodium chromate and potassium chromate, an ionically permeable separator medium between said anode and said depolarizer, said separator medium consisting of paper backing having bound thereto a colloid bibulous in said electrolyte and resistant to hydrolysis in said electrolyte, said colloid being selected from the group consisting of locust bean gum, gum karaya and polyacrylamide resins and being bound to said paper backing by means of a binder resin.
3. The cell of claim 2 wherein said binder resin is dissolved in a low molecular weight organic solvent.
4. In a cell having an anode consisting of aluminum and alloys thereof, and an electrolyte selected from. the group consisting of aluminum chloride, ammonium chr0- mate, aluminum chloride hexahydrate, sodium chromate and potassium chromate, an ionically permeable separator medium bound to said anode, said separator medium comprising a colloid bibulous in said electrolyte and resistant to hydrolysis in said electrolyte, said colloid being selected from the group consisting of locust bean gum, gum karaya and polyacrylamide resins and being bound to the said anode by means of a binder resin.
5. The cell of claim 4 wherein said binder resin is dissolved in a low molecular weight organic solvent.
References Cited in the file of this patent UNITED STATES PATENTS 1,201,481 McGall et a1 Oct. 17, 1916 1,807,875 Robinson June 2, 1931 2,200,301 Ruben May 14, 1940 2,534,336 Cahoon Dec. 19, 1950 2,551,799 Hatfield May 8, 1951 2,796,456 Stokes June 18, 1957 2,927,951 Lindstrom Mar. 8, 1960 FOREIGN PATENTS 541,696 Great Britain Dec. 8, 1941

Claims (1)

1. IN A CELL HAVING AN ANODE CONSISTING OF ALUMINUM AND ALLOYS THEREOF, A DELOLARIZER AND AN ELECTROLYTE SELECTED FROM TH GROUP CONSISTING OF ALUMINUM CHLORIDE, AMMONIUM CHROMATE, ALUMIUNUM CHLORIDE HEXAHYDRATE, SODIUM CHROMATE AND POTASSIUM CHROMATE, AN IONICALLY PERMEABLE SEPARATOR MEDIUM BETWEEN SAID ANODE AND SAID DEPOLARIZER, SAID SEPARATOR MEDIUM BETWEEN SAID ANODE AND SAID BIBULOUS IN SAID SEPARATOR MEDIUM COMPRISING A COLLOID SAID ELECROLYTE, SAID COLLIOD BEING SELECTED FROM THE GROUP CONSISTING OF LOCUST BEAN GUM, GUM KARAYA AND POLYACRYLAMIDE RESINS.
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Cited By (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US3307976A (en) * 1964-11-25 1967-03-07 Aluminum Co Of America Primary cell
US3888700A (en) * 1968-11-01 1975-06-10 Esb Inc Absorbent separator for an electric battery

Citations (8)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US1201481A (en) * 1914-08-12 1916-10-17 New Jersey Patent Co Galvanic battery.
US1807875A (en) * 1926-10-21 1931-06-02 Meriden Gravure Company Method of electroplating and product thereof
US2200301A (en) * 1937-01-22 1940-05-14 Ruben Samuel Potential-producing cell
GB541696A (en) * 1940-06-05 1941-12-08 Major Conrad Lawrence Walsh An improved electrolyte absorbent for primary and secondary batteries
US2534336A (en) * 1944-12-14 1950-12-19 Union Carbide & Carbon Corp Primary galvanic cell
US2551799A (en) * 1946-11-16 1951-05-08 Union Carbide & Carbon Corp Process for lining a metallic dry cell anode
US2796456A (en) * 1955-02-08 1957-06-18 Aluminum Co Of America Primary cell anode
US2927951A (en) * 1954-08-19 1960-03-08 Svenska Ackumulator Ab Hermetically closed storage cell and a method in the manufacture of such cell

Patent Citations (8)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US1201481A (en) * 1914-08-12 1916-10-17 New Jersey Patent Co Galvanic battery.
US1807875A (en) * 1926-10-21 1931-06-02 Meriden Gravure Company Method of electroplating and product thereof
US2200301A (en) * 1937-01-22 1940-05-14 Ruben Samuel Potential-producing cell
GB541696A (en) * 1940-06-05 1941-12-08 Major Conrad Lawrence Walsh An improved electrolyte absorbent for primary and secondary batteries
US2534336A (en) * 1944-12-14 1950-12-19 Union Carbide & Carbon Corp Primary galvanic cell
US2551799A (en) * 1946-11-16 1951-05-08 Union Carbide & Carbon Corp Process for lining a metallic dry cell anode
US2927951A (en) * 1954-08-19 1960-03-08 Svenska Ackumulator Ab Hermetically closed storage cell and a method in the manufacture of such cell
US2796456A (en) * 1955-02-08 1957-06-18 Aluminum Co Of America Primary cell anode

Cited By (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US3307976A (en) * 1964-11-25 1967-03-07 Aluminum Co Of America Primary cell
US3888700A (en) * 1968-11-01 1975-06-10 Esb Inc Absorbent separator for an electric battery

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